Impact of Surface Functionalization on the Quantum Coherence of Nitrogen-Vacancy Centers in Nanodiamonds.

Nanoscale quantum probes such as the nitrogen-vacancy (NV) center in diamonds have demonstrated remarkable sensing capabilities over the past decade as control over fabrication and manipulation of these systems has evolved. The biocompatibility and rich surface chemistry of diamonds has added to the utility of these probes but, as the size of these nanoscale systems is reduced, the surface chemistry of diamond begins to impact the quantum properties of the NV center. In this work, we systematically study the effect of the diamond surface chemistry on the quantum coherence of the NV center in nanodiamonds (NDs) 50 nm in size. Our results show that a borane-reduced diamond surface can on average double the spin relaxation time of individual NV centers in nanodiamonds when compared to thermally oxidized surfaces. Using a combination of infrared and X-ray absorption spectroscopy techniques, we correlate the changes in quantum relaxation rates with the conversion of sp2 carbon to C-O and C-H bonds on the diamond surface. These findings implicate double-bonded carbon species as a dominant source of spin noise for near surface NV centers. The link between the surface chemistry and quantum coherence indicates that through tailored engineering of the surface, the quantum properties and magnetic sensitivity of these nanoscale systems may approach that observed in bulk diamond.

Adsorption differences between low coverage enantiomers of alanine on the chiral Cu{421}R surface.

Chiral separation using heterogeneous methods has long been sought after. Chiral metal surfaces have the potential to make it possible to model these systems using small amino acids, the building blocks for proteins. A comparison of submonolayer concentrations of alanine enantiomers adsorbed onto Cu{421}R has revealed a large geometrical differences between the two molecules as compared to the saturated coverage. Large differences were observed in HR-XPS and NEXAFS and complemented by theoretical DFT calculations. At approximately one third of a monolayer a comparison of the C1s XPS signal showed a shift in the methyl group of more than 300 meV indicating that the two enantiomers are in different chemical environments. NEXAFS spectroscopy confirmed the XPS variations and showed large differences in the orientation of the adsorbed molecules. Our DFT results show that the l-enantiomer is energetically the most stable in the {311} microfacet configuration. In contrast to the full monolayer coverage, these lower coverages showed enhanced selectivity.

Molecular Doping the Topological Dirac Semimetal Na3Bi across the Charge Neutrality Point with F4-TCNQ.

We perform low-temperature transport and high-resolution photoelectron spectroscopy on 20 nm thin film topological Dirac semimetal Na3Bi grown by molecular beam epitaxy. We demonstrate efficient electron depletion ∼10(13) cm(-2) of Na3Bi via vacuum deposition of molecular F4-TCNQ without degrading the sample mobility. For samples with low as-grown n-type doping (1 × 10(12) cm(-2)), F4-TCNQ doping can achieve charge neutrality and even a net p-type doping. Photoelectron spectroscopy and density functional theory are utilized to investigate the behavior of F4-TCNQ on the Na3Bi surface.

Electronic Properties of High-Quality Epitaxial Topological Dirac Semimetal Thin Films.

Topological Dirac semimetals (TDS) are three-dimensional analogues of graphene, with linear electronic dispersions in three dimensions. Nanoscale confinement of TDSs in thin films is a necessary step toward observing the conventional-to-topological quantum phase transition (QPT) with increasing film thickness, gated devices for electric-field control of topological states, and devices with surface-state-dominated transport phenomena. Thin films can also be interfaced with superconductors (realizing a host for Majorana Fermions) or ferromagnets (realizing Weyl Fermions or T-broken topological states). Here we report structural and electrical characterization of large-area epitaxial thin films of TDS Na3Bi on single crystal Al2O3[0001] substrates. Charge carrier mobilities exceeding 6,000 cm(2)/(V s) and carrier densities below 1 × 10(18) cm(-3) are comparable to the best single crystal values. Perpendicular magnetoresistance at low field shows the perfect weak antilocalization behavior expected for Dirac Fermions in the absence of intervalley scattering. At higher fields up to 0.5 T anomalously large quadratic magnetoresistance is observed, indicating that some aspects of the low field magnetotransport (µB < 1) in this TDS are yet to be explained.

Highly chromium contaminant tolerant BaO infiltrated La0.6Sr0.4Co0.2Fe0.8O3-δ cathodes for solid oxide fuel cells.

A BaO infiltrated La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF) cathode shows remarkable tolerance and resistance towards chromium via the formation of BaCrO4 instead of SrCrO4 on the electrode surface, preventing the excess Sr deficiency at the A-site of LSCF perovskite and thus mitigating the Cr poisoning effect.

Manipulating the orientation of an organic adsorbate on silicon: a NEXAFS study of acetophenone on Si(0 0 1).

We investigate the chemical and structural configuration of acetophenone on Si(0 0 1) using synchrotron radiation core-level spectroscopy techniques and density functional theory calculations. Samples were prepared by vapour phase dosing of clean Si(0 0 1) surfaces with acetophenone in ultrahigh vacuum. Near edge x-ray absorption fine structure spectroscopy and photoelectron spectroscopy measurements were made at room temperature as a function of coverage density and post-deposition anneal temperature. We show that the dominant room temperature adsorption structure lies flat on the substrate, while moderate thermal annealing induces the breaking of Si-C bonds between the phenyl ring and the surface resulting in the reorientation of the adsorbate into an upright configuration.

Direct observation of phonon emission from hot electrons: spectral features in diamond secondary electron emission.

In this work we use high-resolution synchrotron-based photoelectron spectroscopy to investigate the low kinetic energy electron emission from two negative electron affinity surfaces of diamond, namely hydrogenated and lithiated diamond. For hydrogen-terminated diamond electron emission below the conduction band minimum (CBM) is clearly observed as a result of phonon emission subsequent to carrier thermalization at the CBM. In the case of lithiated diamond, we find the normal conduction band minimum emission peak is asymmetrically broadened to higher kinetic energies and argue the broadening is a result of ballistic emission from carriers thermalized to the CBM in the bulk well before the onset of band-bending. In both cases the spectra display intensity modulations that are the signature of optical phonon emission as the main mechanism for carrier relaxation. To our knowledge, these measurements represent the first direct observation of hot carrier energy loss via photoemission.